Aerosol Iron from Metal Production as a Secondary Source of Bioaccessible Iron.

Atmospheric iron (Fe) from anthropogenic, lithogenic, and pyrogenic sources contributes to ocean fertilization, climate change, and human health risk. However, significant uncertainties remain in the source apportionment due to a lack of source-specific evaluation of Fe-laden aerosols. Here, the large uncertainties in the model estimates are investigated using different Fe emissions from metal production. The best agreement in the anthropogenic factor of aerosol Fe concentrations with the field data in the downstream region of East Asian outflow (median: 0.026 µg m-3) is obtained with the low case (0.023 µg m-3), whereas the best agreement of aerosol Fe bioaccessibility with field data (4.5%) over oceans south of 45°S is obtained with the high case (4.9%). Our simulation with the low case confirms that anthropogenic aerosols play dominant roles in bioaccessible Fe deposition in the northwestern Pacific, compared to lithogenic sources. Our simulations with higher cases suggest that Fe-containing particles co-emitted with sulfur dioxide from metal production substantially contribute to atmospheric bioaccessible Fe fluxes to the Southern Ocean. These findings highlight that accurate representation of aerosol Fe from metal production is a key to reduce large uncertainties in bioaccessible Fe deposition fluxes to the Southern Ocean (0.7-4.4 Gg Fe year-1).

Asian dust-deposition flux to the subarctic Pacific estimated using single quartz particles.

Iron availability limits marine ecosystem activities in large areas of the ocean. However, the sources and seasonal supply of iron, critically important for controlling surface ocean biogeochemistry and carbon cycling, are poorly understood. The western subarctic Pacific is a high-nutrient and low-chlorophyll region, and despite high concentrations of macronutrients, iron limits phytoplankton production in summer. Here, we determine the seasonal deposition flux of Asian dust using scanning electron microscope-cathodoluminescence analysis of single quartz particles derived from the western subarctic Pacific during 2003-2022 to trace provenance. We found a high (up to 6.9 mg m-2 day-1) deposition flux of Asian dust in May, June, and early July, with an annual average of 1.0 ± 0.2 mg m-2 day-1. The supply of dissolved-iron flux calculated from Asian dust was 0.9 ± 0.3 µg m-2 day-1 during the high productivity season (April-July), which is approximately half that from the deeper part of the ocean, calculated from vertical profiles of dissolved iron. Our study provides a reliable approach for estimating iron supply from dust to the surface ocean that may be critical for sustaining biological productivity under future ocean stratification, which suppresses nutrient supply from the subsurface ocean.

Characteristics of atmospheric black carbon and other aerosol particles over the Arctic Ocean in early autumn 2016: Influence from biomass burning as assessed with observed microphysical properties and model simulations.

We conducted ship-based measurements of marine aerosol particles (number concentration, size distribution, black carbon (BC), autofluorescence property, and PM2.5 composition) and trace gases (ozone (O3) and carbon monoxide (CO)) during a cruise of the R/V Mirai (23 August to 4 October 2016) over the Arctic Ocean, Northwest Pacific Ocean, and Bering Sea. Over the Arctic Ocean at latitudes >70°N, the averaged BC mass concentration was 0.7 ± 1.8 ng/m3, confirming the validity of our previously-reported observations (~1 ng/m3) over the same region during September 2014 and September 2015. The observed levels over the Arctic Ocean need to be used as a benchmark when testing the atmospheric transport models over the ocean, while they are substantially lower than those reported at Barrow (Utqiagvik), a nearby ground-based station. We identified events with elevated BC mass concentrations and CO mixing ratios over the Arctic Ocean and Bering Sea as influenced by biomass burnings, with evidences from elevated levoglucosan levels, mixing states of BC particles, and particle size distributions. With WRF-Chem model simulations, we confirmed Siberian Forest fire plumes traveled over thousands of kilometers and produced substantially high BC and CO levels over the Bering Sea. The ΔBC/ΔCO ratios during these periods were estimated as ~1 ng/m3/ppbv, which are lower than those values reported, indicating that the results might have been affected by the wet removal process during transportation and/or by emission in smoldering conditions.

Light-absorption properties of brown carbon aerosols in the Asian outflow: Implications of a combination of filter and ground remote-sensing observations at Fukue Island, Japan.

Brown carbon (BrC) aerosols have important warming effects on Earth's radiative forcing. However, information on the evolution of the light-absorption properties of BrC aerosols in the Asian outflow region is limited. In this study, we evaluated the light-absorption properties of BrC using in-situ filter measurements and sky radiometer observations of the ground-based remote sensing network SKYradiometer NETwork (SKYNET) made on Fukue Island, western Japan in 2018. The light-absorption coefficient of BrC obtained from filter measurements had a temporal trend similar to that of the ambient concentration of black carbon (BC), indicating that BrC and BC have common combustion sources. The absorption Angstrom exponent in the wavelength range of 340-870 nm derived from the SKYNET observations was 15% higher in spring (1.81 ± 0.30) than through the whole year (1.53 ± 0.50), suggesting that the Asian outflow carries light-absorbing aerosols to Fukue Island and the western North Pacific. After eliminating the contributions of BC, the absorption Angstrom exponent of BrC alone obtained from filter observations had a positive Spearman correlation (rs = 0.77, p < 0.1) with that derived from SKYNET observations but 33% higher values, indicating that the light-absorption properties of BrC were successfully captured using the two methods. Using the atmospheric transport model FLEXPART and fire hotspots obtained from the Visible Infrared Imaging Radiometer Suite product, we identified a high-BrC event related to an air mass originating from regions with consistent fossil fuel combustion and sporadic open biomass burning in central East China. The results of the study may help to clarify the dynamics and climatic effects of BrC aerosols in East Asia.

Dominance of the residential sector in Chinese black carbon emissions as identified from downwind atmospheric observations during the COVID-19 pandemic.

Emissions of black carbon (BC) particles from anthropogenic and natural sources contribute to climate change and human health impacts. Therefore, they need to be accurately quantified to develop an effective mitigation strategy. Although the spread of the emission flux estimates for China have recently narrowed under the constraints of atmospheric observations, consensus has not been reached regarding the dominant emission sector. Here, we quantified the contribution of the residential sector, as 64% (44-82%) in 2019, using the response of the observed atmospheric concentration in the outflowing air during Feb-Mar 2020, with the prevalence of the COVID-19 pandemic and restricted human activities over China. In detail, the BC emission fluxes, estimated after removing effects from meteorological variability, dropped only slightly (- 18%) during Feb-Mar 2020 from the levels in the previous year for selected air masses of Chinese origin, suggesting the contributions from the transport and industry sectors (36%) were smaller than the rest from the residential sector (64%). Carbon monoxide (CO) behaved differently, with larger emission reductions (- 35%) in the period Feb-Mar 2020, suggesting dominance of non-residential (i.e., transport and industry) sectors, which contributed 70% (48-100%) emission during 2019. The estimated BC/CO emission ratio for these sectors will help to further constrain bottom-up emission inventories. We comprehensively provide a clear scientific evidence supporting mitigation policies targeting reduction in residential BC emissions from China by demonstrating the economic feasibility using marginal abatement cost curves.